Organic-Inorganic Hybrid Materials PDF
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O r g a n ic - I n o r g a n ic H y b r id M a t e r ia l s • J e s ú s - M a r ía G a r c ía - M a r t ín e z a n d E m ilia P . C Organic-Inorganic o lla r Hybrid Materials Edited by Jesús-María García-Martínez and Emilia P. Collar Printed Edition of the Special Issue Published in Polymers www.mdpi.com/journal/polymers Organic-Inorganic Hybrid Materials Organic-Inorganic Hybrid Materials Editors Jesu´s-Mar´ıaGarc´ıa-Mart´ınez EmiliaP.Collar MDPI•Basel•Beijing•Wuhan•Barcelona•Belgrade•Manchester•Tokyo•Cluj•Tianjin Editors Jesu´s-Mar´ıaGarc´ıa-Mart´ınez EmiliaP.Collar PolymerEngineeringGroup(GIP) PolymerEngineeringGroup(GIP) PolymerScienceandTechnologyInstitute(ICTP) PolymerScienceandTechnologyInstitute(ICTP) SpanishCouncilforScientificResearch(CSIC) SpanishCouncilforScientificResearch(CSIC) Spain Spain EditorialOffice MDPI St.Alban-Anlage66 4052Basel,Switzerland ThisisareprintofarticlesfromtheSpecialIssuepublishedonlineintheopenaccessjournalPolymers (ISSN2073-4360)(availableat:http://www.mdpi.com). Forcitationpurposes,citeeacharticleindependentlyasindicatedonthearticlepageonlineandas indicatedbelow: LastName,A.A.;LastName,B.B.;LastName,C.C.ArticleTitle. JournalNameYear,VolumeNumber, PageRange. ISBN978-3-0365-1301-0(Hbk) ISBN978-3-0365-1302-7(PDF) ©2021bytheauthors. ArticlesinthisbookareOpenAccessanddistributedundertheCreative Commons Attribution (CC BY) license, which allows users to download, copy and build upon publishedarticles,aslongastheauthorandpublisherareproperlycredited,whichensuresmaximum disseminationandawiderimpactofourpublications. ThebookasawholeisdistributedbyMDPIunderthetermsandconditionsoftheCreativeCommons licenseCCBY-NC-ND. Contents AbouttheEditors ........................................................................................................................................ vii Jesu´s-Mar´ıaGarc´ıa-Mart´ınezandEmiliaP.Collar Organic–InorganicHybridMaterials Reprintedfrom:Polymers2021,13,86,doi:10.3390/polym13010086 . . . . . . . . . . . . . . . . . 1 CoroEcheverrı´a,MiguelRubioandDanielLo´pez Thermo-ReversibleHybridGelsFormedfromtheCombinationofIsotacticPolystyrene and [Fe(II) (4-Octadecyl-1,2,4-Triazole)3(ClO4)2]n Metallo-Organic Polymer: Thermal and ViscoelasticProperties Reprintedfrom:Polymers2019,11,957,doi:10.3390/polym11060957 . . . . . . . . . . . . . . . . . 5 WeiPeng,YingQian,TongZhou,ShenglinYang,JunhongJinandGuangLi Influence of Incorporated Polydimethylsiloxane on Properties of PA66 Fiber and Its FabricPerformance Reprintedfrom:Polymers2019,11,1735,doi:10.3390/polym11111735 . . . . . . . . . . . . . . . . 21 XinxinSheng,SihaoLi,YanfengZhao,DongshengZhai,LiZhangandXiangLu SynergisticEffectsofTwo-DimensionalMXeneandAmmoniumPolyphosphateonEnhancing theFireSafetyofPolyvinylAlcoholCompositeAerogels Reprintedfrom:Polymers2019,11,1964,doi:10.3390/polym11121964 . . . . . . . . . . . . . . . . 31 RosaBarranco-Garc´ıa,Jose´ M.Go´mez-Elvira,JorgeA.Ressia,LidiaQuinzani,EnriqueM. Valle´s,ErnestoPe´rezandMar´ıaL.Cerrada VariationofUltimatePropertiesinExtrudediPP-MesoporousSilicaNanocompositesbyEffect ofiPPConfinementwithintheMesostructures Reprintedfrom:Polymers2020,12,70,doi:10.3390/polym12010070 . . . . . . . . . . . . . . . . . 49 RuiP.C.L.Sousa,Ba´rbaraFerreira,MiguelAzenha,SusanaP.G.Costa,CarlosJ.R.Silva andRitaB.Figueira PDMS Based Hybrid Sol-Gel Materials for Sensing Applications in Alkaline Environments: SynthesisandCharacterization Reprintedfrom:Polymers2020,12,371,doi:10.3390/polym12020371 . . . . . . . . . . . . . . . . . 71 Adria´n Leone´s, Alicia Mujica-Garcia, Marina Patricia Arrieta, Valentina Salaris, Daniel Lopez,Jose´MariaKennyandLauraPeponi OrganicandInorganicPCL-BasedElectrospunFibers Reprintedfrom:Polymers2020,12,1325,doi:10.3390/polym12061325 . . . . . . . . . . . . . . . . 89 SilviaVita,RicoRicotti,AndreaDodero,SilviaVicini,PerBorchardt,EmilianoPinoriand MailaCastellano Rheological, MechanicalandMorphologicalCharacterizationofFillersintheNauticalField: TheRoleofDispersingAgentsonCompositeMaterials Reprintedfrom:Polymers2020,12,1339,doi:10.3390/polym12061339 . . . . . . . . . . . . . . . . 105 NantikanPhuhiangpa,WorachaiPonloa,SareePhongphanphaneeandWirasakSmitthipong Performance of Nano- and Microcalcium Carbonate in Uncrosslinked Natural Rubber Composites:NewResultsofStructure–PropertiesRelationship Reprintedfrom:Polymers2020,12,2002,doi:10.3390/polym12092002 . . . . . . . . . . . . . . . . 117 v Ba`rbaraMico´-Vicent, MarinaRamos, FrancescaLuzi, FrancoDominici, Valentı´nViqueira, LuigiTorre,AlfonsoJime´nez,DeboraPugliaandMarı´aCarmenGarrigo´s EffectofChlorophyllHybridNanopigmentsfromBroccoliWasteonThermomechanicaland ColourBehaviourofPolyester-BasedBionanocomposites Reprintedfrom:Polymers2020,12,2508,doi:10.3390/polym12112508 . . . . . . . . . . . . . . . . 133 Jesu´s-Mar´ıaGarc´ıa-Mart´ınezandEmiliaP.Collar OntheCombinedEffectofBoththeReinforcementandaWasteBasedInterfacialModifieron theMatrixGlassTransitioniniPP/a-PP-pPBMA/MicaComposites Reprintedfrom:Polymers2020,12,2606,doi:10.3390/polym12112606 . . . . . . . . . . . . . . . . 153 YuxiaLiang,XiaonanHuang,LanzhongYao,RuXia,MingCao,QianqianGe,WeibinZhou, JiashengQian,JibinMiaoandBinWu RegulationofPolyvinylAlcohol/SulfonatedNano-TiO2HybridMembranesInterfacePromotes DiffusionDialysis Reprintedfrom:Polymers2021,13,14,doi:10.3390/polym13010014 . . . . . . . . . . . . . . . . . 167 vi About the Editors Jesu´s-Mar´ıa Garc´ıa-Mart´ınez holds a Ph.D. in Chemistry (Chemical Engineering) by the UniversidadComplutensedeMadrid(1995). Additionally, heholdstwoM.Sc. leveldegreesand hascompletedmorethan70highlyspecializedcoursesinindustrialchemistry;polymerscienceand technology; quantitative research; environmental science; materials science and characterization; R+D+i management, modelling of processes; quality systems in R+D+i, educational sciences, philosophyofscience,andsoon. HeisaTenuredScientistattheInstituteofPolymerScienceand Technology(ICTP)oftheSpanishNationalResearchCouncil(CSIC).Since1992,withinthePolymer Engineering Group (GIP), he has co-authored more than 175 scientific and/or technical works in the topics related to polymer engineering, chemical modification of polymers, heterogeneous materials based on polymers, interphases and interfaces, polymer composites blends and alloys, organic-inorganic hybrids materials, polymer recycling, quality, and so on. Dr. Garc´ıa-Mart´ınez has participated in more than 31 research projects financed with either public (national and internationalprograms)orindustrialfunds,andisco-authorofonecurrentlyactiveindustrialpatent onpolymerrecycling. Asanadditionaltasktohisscientificresearch, intheperiod2000–2005, he assumedthepositionofQualityDirectorfortheICTP(CSIC)ISO17025AccreditationProjectofthe ICTP Laboratories (ACiTP) under the auspices of the ICTP (CSIC) Directorate. Additionally, Dr. Garc´ıa-Mart´ınezplaysaveryactiveroleinreviewingtasksforWOSandSCOPUSindexedjournals, withmorethan250reportsinthelastyears. Infact,hehasbeenawardedtwicewiththePublons Reviewer Awards (2018, and 2019), and once with the POLYMERS Outstanding Reviewer Award (2019)fortheseactivities. Since2016,heistheHeadoftheDepartmentofChemistryandProperties ofPolymerMaterialswithintheICTP(CSIC). EmiliaP.Collar, Ph.D.inIndustrialChemistry(U.Complutense, 1986), joinedin1990atthe permanentstaffattheConsejoSuperiordeInvestigacionesCient´ıficas(CSIC),servingasaTenured Scientist, after two-years (1986–88) as CSIC’s postdoc fellow, and one more (1989) as Chemical EngineeringAssistantTeacherattheUniversidadComplutensedeMadrid. AtthePolymerScience andTechnologyInstitute(InstitutodeCienciayTecnolog´ıadePol´ımeros), ICTP/CSIC,sheworks at the Polymer Engineering Group (GIP), founded in 1982 by Prof. O. Laguna, being the GIP’s Headfrom1999. Between1990and2005,shesupervisedsixdoctoralthesesandfivepost-graduate ones,developedunder14researchprojects(publicfundssupported),aswellas18researchcontracts (privatefundssupported),issuing53technicalreportsfordifferentcompanies.From2001to2005,she performedthepositionsofTechnicalDirectorofthePhysicalandMechanicalPropertiesLaboratory, LFM,andDeputy-TechnicalDirectoroftheThermalPropertiesLaboratory,LPT,underthesuccessful ISO17025AccreditationProjectfortheCSIC/ICTP’sLaboratories,ACiTP,commandedbytheICTP’s Head.Authorandco-authorofmorethantwentychaptersonbooks,twocurrentlyactiveindustrial patentsonpolymerrecycling,andmorethanonehundredandfiftyresearchpapersmostlyonSCI Journals,herresearchworklinesdealwithpolymersandenvironmentunderthegeneralframeof heterogeneousmaterialsbasedonpolymers(PolymersandEnvironment; PolymerRecycling; Polymer Blends; Composites; Interface Optimization; Interfacial Agents; Chemical Modification of Polymers; Blend Technologies;MorphologyandModeling).From2006todate,shehasparticipatedinthreeSpanishpublic fundedresearchprojectsandoneEUpublicfundedprojectunderits7thFrameworkProgram. vii polymers Editorial Organic–Inorganic Hybrid Materials Jesús-MaríaGarcía-Martínez*andEmiliaP.Collar* PolymerEngineeringGroup(GIP),PolymerScienceandTechnologyInstitute(ICTP), SpanishCouncilforScientificResearch(CSIC),C/JuandelaCierva,3,28006Madrid,Spain * Correspondence:[email protected](J.-M.G.-M.);[email protected](E.P.C.) AccordingtotheIUPAC(InternationalUnionofPureandAppliedChemistry),ahy- bridmaterialisthatcomposedofanintimatemixtureofinorganiccomponents,organic components,orbothtypesofcomponentswhichusuallyinterpenetrateonscalesofless than1μm[1].Thisdefinitionmatchesthesubjectofallthearticlespublishedinthisspecial issue.Thus,theconceptoforganic–inorganichybridmaterialscanbeappliedtoabroad numberofapproaches.Inthesameway,theso-calledorganic–inorganicmaterialscanbe revealedasmulti-componentcompoundshavingatleastoneoftheirorganic(thepolymer) orinorganiccomponentinthesub-micrometricand,moreusually,inthenano-metricsize domain[2].Further,theorganic–inorganichybridsystemscanbeclassifiedintotwoclasses namedclassIandClassII,dependingoniftheinteractionofthephasesisweakorstrong, respectively[2].Thelatterdependsonthetypeofinteractions:VanderWaals,hydrogen, electrostatic,andotherinteractionsforClassI,andduetorealchemicalbondsbetween phases(ClassII),thecoexistenceofbothtypesofinteractions(IandII)inthesamesystemis possible[2].Insuchascenario,thisissueincludesawiderangeoftopicscoveringthesedef- initions.Consequently,theorganic–inorganicmaterialsarerevealedasmulti-component compoundshavingatleastoneoftheirorganic(thepolymer)orinorganiccomponent inthenano-metricsizedomain,andusuallyoffersmuchbetterperformancethantheir non-hybridcounterparts[2–6]. (cid:2)(cid:3)(cid:4)(cid:2)(cid:5)(cid:6)(cid:7)(cid:8)(cid:9) (cid:2)(cid:3)(cid:4)(cid:5)(cid:6)(cid:7)(cid:8) Undertheabove-mentionedpremises,thisspecialissuecompiles11articleswrittenby expertsinthefieldandaredevotedtotheverydifferentapproachescoexistinginthefield. Citation:García-Martínez,J.-M.; Inthiscontext,thefirstarticlebyEcheverría,Rubio,andLópez[7]studiesofthermo- Collar,E.P.Organic–InorganicHybrid reversibleorganic–inorganichybridgelsbymeansofthermalandviscolesticproperties. Materials.Polymers2021,13,86. Forsuchpurposes,theyusedsynthetizedhybridthermo-reversiblegelsbycombining https://doi.org/10.3390/ a metallo-organic polymer and isotactic polystyrene with the purpose of solving the polym13010086 poormechanicalpropertiesofthesetypesofcompounds. Theywereabletodetermine Received:24December2020 threetransitionsuponheating(monotectictransitionoftheiPSgel,meltingoftheiPSgel, Accepted:25December2020 andmeltingofthemetal-organicpolymergel)suggestingthatthetwopolymersareformed Published:28December2020 independentlyinthehybridgel,concludingthatthesehybridgelsareinterpenetrated organic/metallo-organicnetworks. Publisher’sNote: MDPIstaysneu- Lietal.[8]investigatedtheinfluenceofincorporatingpolydimethylsiloxaneonthe tralwithregardtojurisdictionalclaims propertiesofPA66fiberfabrics,obtainedbymeltblendspinning,byproducingfiberswith inpublishedmapsandinstitutional excellentmechanicalpropertiesandreducedhotshrinkage,withoutremarkableeffecton affiliations. crystallizationandmeltingbehaviorofPA66.Thus,theeffectoftheadditiveonthesurface tensionsuggeststheantifouling,waterproof,andstain-resistantabilityofthefiberandits fabric.Theseresultsarecomparedwithsilicon-coatedfibers,resultingintheproposition bytheauthorsofthecompoundshavingmanypropertiesbesidesbeingecofriendly. Copyright:©2020bytheauthors.Li- Relatedtothehottopicoffireresistancematerials,Sheng,Lu,andco-workersreport censeeMDPI,Basel,Switzerland.This astudyaboutit[9].So,thisarticleisdevotedtofireandsmokesuppressionsofpolyvinyl articleisanopenaccessarticledistributed alcohol(PVA)aerogelsinordertoavoidthefirehazardthattheypresent. Forthispur- underthetermsandconditionsofthe CreativeCommonsAttribution(CCBY) pose,theauthorsuseda2Dtransition-metalcarbideforenhancingtheflame-retardant license(https://creativecommons.org/ performanceofPVA/ammoniumpolyphosphate-basedcomposites.Theresultsdemon- licenses/by/4.0/). stratedthatthepresenceofthecarbideinlowamountscanboosttheflameretardanceof 1 Polymers2021,13,86.https://doi.org/10.3390/polym13010086 https://www.mdpi.com/journal/polymers Polymers2021,13,86 thecompositesevenastopassasV-0rated.Furthermore,theauthorsdemonstratethat thepresenceofthecarbidegreatlyreducesthereleaseofheatandsmoke,provingthe synergisticeffectoftheammoniumphosphateandthecarbideusedfortheobjectiveof thestudy. Aninvestigationaboutthechangesobservedontheultimatepropertiesofisopropylene– mesoporoussilicananocompositesobtainedbyextrusioncausedbytheeffectofthepoly- mersconfinementwithinthemesostructuresisthesubjectofthearticlebyCerradaand workinggroup[10].Thestudyconcludesthekeyroleofporesizeintheconfinementof iPPchainswithinthenanometricmesostructuresofthesilicasused,affectingthethermal stabilityandtheultimatepropertiesofthematerials.Themainconclusionsofthework weretherelatedeffectofthesilicaonthepolypropyleneobservedthroughthedegradation andtherheologicalbehaviorofthecomposites,whichisexplainedbyvariationsinthe inclusionofthepolymerchainswithinthemesostructuresofthesilicasused.Thelatter wasdemonstratedbysynchrotronSAXSmeasurements. Sincethecarbonationofconcreteisaprimeproblemincivilengineering,thepaperby Sousa,Ferreira,andco-workers[11]isrelatedtothereductionofthisconcretedegradation bytheeffectoforganic–inorganichybridfilmsforthepotentialfunctionalizationofoptical fibersensorstobeappliedinconcretestructures. Virginfilmsandthosedopedwith phenolphthaleinwerecharacterizedbyaseriesoftechniquesandtheresultsobtained werehighlypromisingregardingthepropertiesunderhighalkalinescenarioscausing concretecarbonation. Byconsideringtheincreasingimportanceofadditiveprocessing,theworkbyPeponi etal.[12]isfocusedonthefabricationoforganicandinorganicpoly(e-caprolactone)- basedelectrospunfibersinordertoobtaindifferentnanocompositematsbasedonpoly(e- caprolactone),PCL,reinforcedwithaseriesofbothorganicandinorganicnanoparticles (just1%). Asorganicparticles, theauthorsusedcellulosenanocrystals(producedby them)andcommercialchitosanandgraphene,whiletheinorganiconesweresilverand hydroxyapatiteparticles.Theauthorsfoundnoappreciabledifferencesintermsofthermal parameters. The authors conclude that while the flexibility of the mats increases for whatevertypeofparticleincorporated,thestiffnessofthesystemincreasesonlyinthecase ofsilverorgrapheneparticleispresentinthemat. Theeffectofthedispersingagentswithanionicorstericactionontheinteractions betweenhollowglassmicrospheresandanepoxy-polyamideresinoncompositematerials fornauticalapplicationsarestudiedbyDodero,Vicini,andcolleagues[13].Thecomposites areevaluatedbymeansoftherheologyoftheun-crosslinkedmaterialaswellasmechanical andmorphologicalpropertiesofthecrosslinkedcomposites.Theauthorsconcludethat stericdispersingagentsoffermuchbettercompatibilitythanioniconesbasedontheir hindrancecapability,andsoabetter-performingcompositewithaless-markedPayneeffect isobtained.Theauthorsclaimtobethepioneersinstudyingtheroleofdispersingagents forthistypeofmaterialincomparisontothemerelyempiricalapproachesfollowedforthe preparationoffillersforthistypeofcomposite. Smitthipongandcoworkers[14]studiedtheperformanceofnano-andmicro-calcium carbonatefillersinthefinalpropertiesofun-crosslinkednaturalrubbercompounds,bypay- ingattentionthehighcostreductionforindustryandthehalfreinforcingcharacterof thistypeoffillerspromotingbettermechanicalproperties. Theauthorsfoundasimilar tendencyofresultswiththeindependenceofthenanoormicrocharacterofthenano-filler used;theyalsoshowtheimportanceandinfluenceofthespecificsurfacearea.However, theauthorsconcludetheeffectofthespecificsurfaceareaonthefinalproperties,aswellas thetheoreticalmodelswhichagreewiththeresults.Additionally,theyshowed(through time–temperaturesuperpositionmastercurves)wherethehigherfilledcompositesex- hibited lower free volume. Finally, they conclude about the real possibility of using nano-calciumcarbonatematerialfortheproductionoftailorrubber-basedproducts. Sincebio-basednanocompositeshaveemergedasahottopic,Garrigos,Puglia,andcol- leagues[15]havestudiedtheeffectofchlorophyllhybridnanopigmentsobtainedbycom- 2 Polymers2021,13,86 biningchlorophylldye(obtainedfromagro-foodwastes),calcinedhydrotalcite,andmont- morillonitenanoclay,onthefinalcolorandthermomechanicalproperties,byusingstatisti- caldesignofexperiments,DOEs.Inthisway,theauthorswerecapableofidentifyingthe moreimportantparametersinfluencingthemechanical,thermal,structural,morphological, andcolorpropertiesofthebionanocompositesstudied.Hence,thepotentialuseofgreen naturaldyesfrombroccoliwastes,adsorbedintonanoclays,havebeenproventobevery interestinginthedevelopmentofnaturallycoloredbionanocomposites. Attending to the fact that the interphase between the organic and the inorganic componentsofthehybridmaterialiswhatgovernstheirultimatebehavior,García-Martínez andCollar[16]investigatedthecombinedeffectofthereinforcementandtheinterfacial agentinapolypropylene-basedcomposite.Inthearticle,theauthorsstudiedmicaplatelets andapolymerwasteinterfacialmodifierconsistingofagraftedatacticpolypropylenewith attachedp-phenylen-bis-maleamicacidpolargroups,bypayingattentiontothechangesof theglasstransitiontemperature.ByusingBox–Wilsonexperimentaldesigns,thearticle focusesonthepredictionofhowthisparameterchangesasafunctionofboththeinterfacial agentandthenano-reinforcementbytakingintoconsiderationthecomplexcharacterof theiPP/aPP-pPBMA/micasystem,whereintheinteractionbetweenthecomponentswill definethefinalbehavior,andthattheglasstransitionisadesignthresholdfortheultimate propertiesofpartsbasedinthistypeoforganic–inorganichybridmaterials.Hence,thefinal purposeoftheworkisthepredictionandinterpretationoftheeffectofbothvariables onthiskeyparameter, beingidentifiedthesamecriticalpointsasbyotherproperties suchasflexural,tensile,impact,andthermalproperties,asdeterminedpreviouslyby theauthors[16]. Finally,byfocusingtheattentiononthefactthatistheadjustmentoftheorganic– inorganic interfacial chemical environment which plays a key role for the separation performanceofcompositematerials,Miau,Wuetal.[17]focusedtheirattentiononthe regulationabouthowapolyvinylalcohol/sulfonatednano-TiO2hybridmembranesinter- facepromotesdiffusiondialysis.Forsuchpurposes,theauthorsinvestigatedthebehavior ofaseriesofhybridmembranesfabricatedbycombiningpolyvinylalcohol(PVA)and sulfonatednano-TiO2(SNT).Infact,theyregulatetheeffectsoftheinterfacialchemicalsur- roundingsoniontransferasafunctionoftheSNTcontenttoaffectthedialysiscoefficients ofboththehydroxylionsandtheseparationfactorsinordertobeofanadequateinterval astomakethesulfonicgroupsintheinterfacialregionsandthehydroxylgroupspresent inthePVAmainchain.Thiscanhaveimportantrolesduringthetransportofsodiumand hydroxylions.Moreover,theauthorsidentifiedamembranewithoptimalperformancein thecaseof3%ofSNT. Heterogeneousmaterialsbasedonorganicpolymers(asawholeorasapart)can playanessentialrolesinthefightagainstCOVID-19.Infact,theycanbekeymaterialsfor fabricatingpreventiveandisolationclothingforthemedicalteamsinclosecontactwith illpatients,forlifesupportequipment,containment,andtransportthereof.Additionally, organic–inorganichybridmaterialsremaintherealmforotherdiverseapplicationssuchas controlleddosingofdrugs,membranesystems,multi-componentpackaging,andamyriad ofaccessoriesandsanitaryitemsingeneral. Thechallengeofcontinuallyattendingto newdemandsremains.Thelatterconstitutestheprimemotivationandconcernforhybrid materialsresearch.Thisextensivelyappliestotheworkscompiledinthisspecialissue. Wethankalltheauthorsfortheircontributionsandencouragethemtopursuewith theirresearch. Funding:Thisresearchreceivednoexternalfunding. ConflictsofInterest:Theauthorsdeclarenoconflictofinterest. 3
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